Probing free-carrier and exciton dynamics in a bulk semiconductor with two-dimensional electronic spectroscopy

Bulk semiconductors; Energy resolutions; Exciton dynamics; Femtoseconds; Free carriers; Free excitons; Free-carrier dynamics; MeV energy; Two-dimensional electronic spectroscopies; Ultra-fast dynamics; Electronic, Optical and Magnetic Materials; Condensed Matter Physics

Abstract :

[en] We employ partially collinear two-dimensional electronic spectroscopy to disentangle precisely the ultrafast dynamics of excitons and free carriers in gallium selenide. Femtosecond temporal and meV energy resolution in the visible spectral region allows us to observe ultrafast bleaching at the exciton resonance with a relaxation time of 112 fs that corresponds to the thermal dissociation of excitons at room temperature, and is orders of magnitude faster than carrier relaxation in the bulk crystal. Our method is applicable to other functional materials, two-dimensional systems, and nanostructures.

Disciplines :

Physics

Author, co-author :

ALLERBECK, Jonas ; University of Luxembourg > Faculty of Science, Technology and Medicine > Department of Physics and Materials Science > Team Daniele BRIDA ; University of Konstanz, Konstanz, Germany

DECKERT, Thomas ; University of Luxembourg > Faculty of Science, Technology and Medicine (FSTM) > Department of Physics and Materials Science (DPHYMS)

Spitzner, Laurens; University of Konstanz, Konstanz, Germany

BRIDA, Daniele ; University of Luxembourg > Faculty of Science, Technology and Medicine (FSTM) > Department of Physics and Materials Science (DPHYMS) ; University of Konstanz, Konstanz, Germany

External co-authors :

yes

Language :

English

Title :

Probing free-carrier and exciton dynamics in a bulk semiconductor with two-dimensional electronic spectroscopy

Publication date :

15 November 2021

Journal title :

Physical Review. B

ISSN :

2469-9950

eISSN :

2469-9969

Publisher :

American Physical Society

Volume :

104

Issue :

Peer reviewed :

Peer Reviewed verified by ORBi

Additional URL :

https://link.aps.org/article/10.1103/PhysRevB.104.L201202

Funders :

Deutsche Forschungsgemeinschaft
European Regional Development Fund

Funding text :

We gratefully acknowledge scientific discussion with Dr. A. Leitenstorfer. This work was supported by the Emmy Noether Program of the DFG (Grant No. BR 5030/1-1) and the FEDER Program (Grant No. 2017-03-022-19 “Lux-Ultra-Fast”).

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since 28 September 2023

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Bibliography

K. S. Novoselov, A. Mishchenko, A. Carvalho, and A. H. Castro Neto, 2D materials and van der waals heterostructures, Science (80-.). 353, aac9439 (2016) 10.1126/science.aac9439.
J. Cheng, C. Wang, X. Zou, and L. Liao, Recent advances in optoelectronic devices based on 2D materials and their heterostructures, Adv. Opt. Mater. 7, 1800441 (2019) 10.1002/adom.201800441.
E. Cassette, J. C. Dean, and G. D. Scholes, Two-Dimensional visible spectroscopy for studying colloidal semiconductor nanocrystals, Small 12, 2234 (2016) 10.1002/smll.201502733.
A. Grupp, A. Budweg, M. P. Fischer, J. Allerbeck, G. Soavi, A. Leitenstorfer, and D. Brida, Broadly tunable ultrafast pump-probe system operating at multi-KHz repetition rate, J. Opt. 20, 014005 (2018) 10.1088/2040-8986/aa9b07.
S. T. Cundiff and S. Mukamel, Multidimensional coherent spectroscopy, Physics Today 66(7), 44 (2013) 10.1063/PT.3.2047.
P. Hamm and M. T. Zanni, Concepts and Methods of 2D Infrared Spectroscopy (Cambridge University Press, Cambridge, UK, 2011).
R. M. Hochstrasser, Two-Dimensional spectroscopy at infrared and optical frequencies, Proc. Natl. Acad. Sci. USA 104, 14190 (2007) 10.1073/pnas.0704079104.
D. B. Turner, Y. Hassan, and G. D. Scholes, Exciton superposition states in CdSe nanocrystals measured using broadband Two-Dimensional electronic spectroscopy, Nano Lett. 12, 880 (2012) 10.1021/nl2039502.
L. Guo, M. Wu, T. Cao, D. M. Monahan, Y. H. Lee, S. G. Louie, and G. R. Fleming, Exchange-driven intravalley mixing of excitons in monolayer transition metal dichalcogenides, Nat. Phys. 15, 228 (2019) 10.1038/s41567-018-0362-y.
S. T. Cundiff, Coherent spectroscopy of semiconductors, Opt. Express 16, 4639 (2008) 10.1364/OE.16.004639.
S. T. Cundiff, Optical two-dimensional fourier transform spectroscopy of semiconductor nanostructures [invited], J. Opt. Soc. Am. B 29, A69 (2012) 10.1364/JOSAB.29.000A69.
X. Li, T. Zhang, C. N. Borca, and S. T. Cundiff, Many-Body Interactions In Semiconductors Probed By Optical Two-Dimensional Fourier Transform Spectroscopy, Phys. Rev. Lett. 96, 057406 (2006) 10.1103/PhysRevLett.96.057406.
E. Cassette, R. D. Pensack, B. Mahler, and G. D. Scholes, Room-temperature exciton coherence and dephasing in two-dimensional nanostructures, Nat. Commun. 6, 6086 (2015) 10.1038/ncomms7086.
J. M. Richter, F. Branchi, F. Valduga De Almeida Camargo, B. Zhao, R. H. Friend, G. Cerullo, and F. Deschler, Ultrafast carrier thermalization in lead iodide perovskite probed with two-dimensional electronic spectroscopy, Nat. Commun. 8, 376 (2017) 10.1038/s41467-017-00546-z.
A. Jha, H. G. Duan, V. Tiwari, P. K. Nayak, H. J. Snaith, M. Thorwart, and R. J. Dwayne Miller, Direct observation of ultrafast exciton dissociation in lead iodide perovskite by 2d electronic spectroscopy, ACS Photonics 5, 852 (2018) 10.1021/acsphotonics.7b01025.
A. De Sio, F. Troiani, M. Maiuri, J. Réhault, E. Sommer, J. Lim, S. F. Huelga, M. B. Plenio, C. A. Rozzi, G. Cerullo, E. Molinari, and C. Lienau, Tracking the coherent generation of polaron pairs in conjugated polymers, Nat. Commun. 7, 13742 (2016) 10.1038/ncomms13742.
A. DeSio and C. Lienau, Vibronic coupling in organic semiconductors for photovoltaics, Phys. Chem. Chem. Phys. 19, 18813 (2017) 10.1039/C7CP03007J.
F. Milota, J. Sperling, A. Nemeth, T. Mančal, and H. F. Kauffmann, Two-dimensional electronic spectroscopy of molecular excitons, Acc. Chem. Res. 42, 1364 (2009) 10.1021/ar800282e.
F. Junginger, A. Sell, O. Schubert, B. Mayer, D. Brida, M. Marangoni, G. Cerullo, A. Leitenstorfer, and R. Huber, Single-cycle multiterahertz transients with peak fields above 10 MV/Cm, Opt. Lett. 35, 2645 (2010) 10.1364/OL.35.002645.
O. Schubert, M. Hohenleutner, F. Langer, B. Urbanek, C. Lange, U. Huttner, D. Golde, T. Meier, M. Kira, S. W. Koch, and R. Huber, Sub-cycle control of terahertz high-harmonic generation by dynamical bloch oscillations, Nat. Photonics 8, 119 (2014) 10.1038/nphoton.2013.349.
K. R. Allakhverdiev, M. Ö. Yetis, S. Özbek, T. K. Baykara, and E. Y. Salaev, Effective nonlinear gase crystal. optical properties and applications, Laser Phys. 19, 1092 (2009) 10.1134/S1054660X09050375.
P. Hu, Z. Wen, L. Wang, P. Tan, and K. Xiao, Synthesis of few-layer gase nanosheets for high performance photodetectors, ACS Nano 6, 5988 (2012) 10.1021/nn300889c.
Y. Cao, K. Cai, P. Hu, L. Zhao, T. Yan, W. Luo, X. Zhang, X. Wu, K. Wang, and H. Zheng, Strong enhancement of photoresponsivity with shrinking the electrodes spacing in few layer GaSe photodetectors, Sci. Rep. 5, 08130 (2015) 10.1038/srep08130.
A. Budweg, D. Yadav, A. Grupp, A. Leitenstorfer, M. Trushin, F. Pauly, and D. Brida, Control of excitonic absorption by thickness variation in Few-Layer GaSe, Phys. Rev. B 100, 045404 (2019) 10.1103/PhysRevB.100.045404.
R. Longuinhos and J. Ribeiro-Soares, Ultra-weak interlayer coupling in two-dimensional gallium selenide, Phys. Chem. Chem. Phys. 18, 25401 (2016) 10.1039/C6CP03806A.
D. J. Late, B. Liu, J. Luo, A. Yan, H. S. S. R. Matte, M. Grayson, C. N. R. Rao, and V. P. Dravid, GaS and GaSe ultrathin layer transistors, Adv. Mater. 24, 3549 (2012) 10.1002/adma.201201361.
P. Dey, J. Paul, G. Moody, C. E. Stevens, N. Glikin, Z. D. Kovalyuk, Z. R. Kudrynskyi, A. H. Romero, A. Cantarero, D. J. Hilton, and D. Karaiskaj, Biexciton formation and exciton coherent coupling in layered GaSe, J. Chem. Phys. 142, 212422 (2015) 10.1063/1.4917169.
D. Brida, C. Manzoni, and G. Cerullo, Phase-locked pulses for two-dimensional spectroscopy by a birefringent delay line, Opt. Lett. 37, 3027 (2012) 10.1364/OL.37.003027.
M. Schlüter, J. Camassel, S. Kohn, J. P. Voitchovsky, Y. R. Shen, and M. L. Cohen, Optical properties of GaSe and Ga-Sx-Se(1-x) mixed crystals, Phys. Rev. B 13, 3534 (1976) 10.1103/PhysRevB.13.3534.
R. LeToullec, N. Piccioli, and J. C. Chervin, Optical properties of the band-edge exciton in GaSe crystals at 10 K, Phys. Rev. B 22, 6162 (1980) 10.1103/PhysRevB.22.6162.
J. V. McCanny and R. B. Murray, The band structures of Gallium and Indium selenide, J. Phys. C: Solid State Phys. 10, 1211 (1977) 10.1088/0022-3719/10/8/022.
A. M. Bakiev, Y. V. Vandyshev, G. S. Volkov, V. S. Dneprovskil, Z. D. Kovalyuk, A. R. Lesiv, S. V. Savinov, and A. I. Furtichev, Screening of excitons in semiconductor GaSe, Fiz. Tverd. Tela 28, 1035 (1986)
A. M. Bakiev, Y. V. Vandyshev, G. S. Volkov, V. S. Dneprovskil, Z. D. Kovalyuk, A. R. Lesiv, S. V. Savinov, and A. I. Furtichev, [Sov. Phys. Solid State 28, 579 (1986)].
D. C. Reynolds, D. C. Look, and B. Jogai, Combined effects of screening and band gap renormalization on the energy of optical transitions in ZnO and GaN, J. Appl. Phys. 88, 5760 (2000) 10.1063/1.1320026.
B. Mayer, C. Schmidt, J. Bühler, D. V. Seletskiy, D. Brida, A. Pashkin, and A. Leitenstorfer, Sub-cycle slicing of phase-locked and intense mid-infrared transients, New J. Phys. 16, 063033 (2014) 10.1088/1367-2630/16/6/063033.
P. C. Becker, H. L. Fragnito, C. H. B. Cruz, R. L. Fork, J. E. Cunningham, J. E. Henry, and C. V. Shank, Femtosecond Photon Echoes From Band-To-Band Transitions in GaAs, Phys. Rev. Lett. 61, 1647 (1988) 10.1103/PhysRevLett.61.1647.
S. L. Sewall, R. R. Cooney, K. E. H. Anderson, E. A. Dias, and P. Kambhampati, State-to-state exciton dynamics in semiconductor quantum dots, Phys. Rev. B 74, 235328 (2006) 10.1103/PhysRevB.74.235328.
Y. Yan, G. Chen, and P. G. Van Patten, Ultrafast exciton dynamics in CdTe nanocrystals and Core/Shell CdTe/CdS nanocrystals, J. Phys. Chem. C 115, 22717 (2011) 10.1021/jp204420q.
J. Madéo, M. K. L. Man, C. Sahoo, M. Campbell, V. Pareek, E. L. Wong, A. Al-Mahboob, N. S. Chan, A. Karmakar, B. M. K. Mariserla, X. Li, T. F. Heinz, T. Cao, and K. M. Dani, Directly visualizing the momentum-forbidden dark excitons and their dynamics in atomically thin semiconductors, Science (80-.). 370, 1199 (2020) 10.1126/science.aba1029.
H. Wang, K. Ferrio, D. G. Steel, Y. Z. Hu, R. Binder, and S. W. Koch, Transient Nonlinear Optical Response From Excitation Induced Dephasing in GaAs, Phys. Rev. Lett. 71, 1261 (1993) 10.1103/PhysRevLett.71.1261.
D. B. Turner, P. Wen, D. H. Arias, K. A. Nelson, H. Li, G. Moody, M. E. Siemens, S. T. Cundiff, X. Li, T. Zhang, C. N. Borca, and S. T. Cundiff, Persistent Exciton-Type Many-Body Interactions in GaAs Quantum Wells Measured Using Two-Dimensional Optical Spectroscopy, Phys. Rev. B 85, 201303 (R) (2012) 10.1103/PhysRevB.85.201303.
V. Capozzi, L. Pavesi, and J. L. Staehli, Exciton-carrier scattering in gallium selenide, Phys. Rev. B 47, 6340 (1993) 10.1103/PhysRevB.47.6340.